涂层组分对堇青石脱硝催化剂性能的影响

doi:10.16085/j.issn.1000-6613.2018-0554

化工进展 ›› 2019, Vol. 38 ›› Issue (03): 1411-1418.DOI: 10.16085/j.issn.1000-6613.2018-0554

涂层组分对堇青石脱硝催化剂性能的影响

金其奇(),谢峻林,李凤祥,齐凯,方德(),何峰

武汉理工大学硅酸盐建筑材料国家重点实验室，湖北武汉 430070

收稿日期:2018-03-19 修回日期:2018-08-27 出版日期:2019-03-05 发布日期:2019-03-05
通讯作者: 方德
作者简介:金其奇（1993—），女，硕士研究生，研究方向为烟气脱硝。E-mail：457615508@qq.com。|方德，博士，实验师，研究方向为燃料燃烧及烟气处理。E-mail：fangde0914@163.com。
基金资助:
国家重点研发计划专项(2017YFB0304304)

Performance of structured cordierite catalysts with different coatings for NH₃-SCR

Qiqi JIN(),Junlin XIE,Fengxiang LI,Kai QI,De FANG(),Feng HE

State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070，Hubei, China

Received:2018-03-19 Revised:2018-08-27 Online:2019-03-05 Published:2019-03-05
Contact: De FANG

摘要/Abstract

摘要：

为了探究涂层组分对整体式低温选择性催化还原（SCR）脱硝催化剂性能的影响，本文使用锰氧化物（MnO _x ）、氧化物涂层（TiO₂、SiO₂及Al₂O₃）、堇青石（CC）基体制备整体式涂层催化剂，考察催化剂牢固度以及脱硝活性。结果表明：在200℃ 时，对于MnO _x /Al₂O₃/CC催化剂，MnO _x 负载率为6%（质量分数）时脱硝效率最高为95%；对于MnO _x /TiO₂/CC，负载率为6%~12%时脱硝效率相差不大，为75%左右；对于MnO _x /SiO₂/CC，负载率12%时脱硝效率80%。样品牢固度排列顺序如下：MnO _x /Al₂O₃/CC > MnO _x /SiO₂/CC > MnO _x / TiO₂ /CC。通过BET、SEM、TG、Raman、H₂-TPR等测试与分析方法发现：影响催化剂性能的因素主要为活性组分MnO _x 状态以及载体性能的差异。Al₂O₃涂层比表面积适中，作为载体活性好；SiO₂涂层虽然比表面积大、牢固度好，但作为载体活性差；TiO₂作为涂层比表面积较小，溶胶中溶剂挥发快使得涂层表面不均匀。

关键词: 选择催化还原, 催化剂, 载体, 锰氧化物, 溶胶凝胶法

Abstract:

In order to explore the influence of coating components on the performance of monolithic SCR denitration catalysts, manganese oxide (MnO _x ), oxides (TiO₂, SiO₂, and Al₂O₃) coatings and Honeycomb Cordierite (CC) substrate were selected to prepare structured coating catalysts, and the firmness and the denitrification activity of the catalysts were investigated. The denitration results showed that, for MnO _x /Al₂O₃/CC catalysts, the denitrification efficiency at 200℃ was up to 95% when MnO _x loading amount was 6%. The efficiency was about 75% for MnO _x /TiO₂/CC as the loading was from 6% to 12% and it was 80% with 12% loading for the MnO _x /SiO₂/CC. The sample firmness was in the order: MnO _x /Al₂O₃/CC>MnO _x /SiO₂/CC>MnO _x /TiO₂/CC. Through BET, SEM, TG, Raman, H₂-TPR and other analysis methods, it was found that the differences between the state of active component MnO _x and the performance of the carrier were the main influence factors on the performance of catalysts. The Al₂O₃ coating had moderate specific surface area, and showed good activity as carrier. SiO₂ coating had high specific surface area and good firmness, but it acted poorly as carrier. TiO₂ had relatively small specific surface area, and the solvent evaporation in the sol was fast, resulting in an uneven coating surface uneven.

Key words: selective catalytic reduction, catalyst, support, manganese oxide _x , sol-gel method

中图分类号:

TQ426.65

金其奇,谢峻林,李凤祥,齐凯,方德,何峰. 涂层组分对堇青石脱硝催化剂性能的影响[J]. 化工进展, 2019, 38(03): 1411-1418.

Qiqi JIN,Junlin XIE,Fengxiang LI,Kai QI,De FANG,Feng HE. Performance of structured cordierite catalysts with different coatings for NH₃-SCR[J]. Chemical Industry and Engineering Progress, 2019, 38(03): 1411-1418.

图/表 7

图1 工艺流程图

图2 涂层XRD谱图

图3 催化剂样品表征图谱

表1 不同试样的比表面积

样品	比表面积(S _BET)/m²·g^-1
CC	0.65
Al₂O₃/CC	15.6
TiO₂/CC	10.5
SiO₂/CC	21.2
MnO _x /Al₂O₃/CC	13.2
MnO _x /TiO₂/CC	9.3
MnO _x /SiO₂/CC	18.4

图4 催化剂样品的SEM图

图5 MnO x 负载率与脱落率（Q）的关系图

图6 不同MnO x 负载量的催化剂样品的脱硝性能

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涂层组分对堇青石脱硝催化剂性能的影响

Performance of structured cordierite catalysts with different coatings for NH₃-SCR

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涂层组分对堇青石脱硝催化剂性能的影响

Performance of structured cordierite catalysts with different coatings for NH3-SCR

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Performance of structured cordierite catalysts with different coatings for NH₃-SCR